Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand ...Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)reduction.The results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand modulation.Compared with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and CH_(4).The CO and CH_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.展开更多
The presence of toxic elements in manganese slag(MSG)poses a threat to the environment due to potential pollution.Utilizing CO_(2) curing on MS offers a promising approach to immobilize toxic substances within this ma...The presence of toxic elements in manganese slag(MSG)poses a threat to the environment due to potential pollution.Utilizing CO_(2) curing on MS offers a promising approach to immobilize toxic substances within this material,thereby mitigating their release into the natural surroundings.This study investigates the impact of CO_(2) cured MS on various rheological parameters,including slump flow,plastic viscosity(η),and yield shear stress(τ).Additionally,it assesses flexural and compressive strengths(f_(t) and f_(cu)),drying shrinkage rates(DSR),durability indicators(chloride ion migration coefficient(CMC),carbonization depth(CD)),and the leaching behavior of heavy metal elements.Microscopic examination via scanning electron microscopy(SEM)is employed to elucidate the underlying mechanisms.The results indicate that CO_(2) curing significantly enhances the slump flow of ultra-high performance concrete(UHPC)by up to 51.2%.Moreover,it reduces UHPC’sηandτby rates ranging from 0%to 52.7%and 0%to 40.2%,respectively.The DSR exhibits a linear increase corresponding to the mass ratio of CO_(2) cured MS.Furthermore,CO_(2) curing enhances both f_(t) and f_(cu) of UHPC by up to 28.7%and 17.6%,respectively.The electrical resistance is also improved,showing an increase of up to 53.7%.The relationship between mechanical strengths and electrical resistance follows a cubic relationship.The CO_(2) cured MS demonstrates a notable decrease in the CMC and CD by rates ranging from 0%to 52.6%and 0%to 26.1%,respectively.The reductions of leached chromium(Cr)and manganese(Mn)are up to 576.3%and 1312.7%,respectively.Overall,CO_(2) curing also enhances the compactness of UHPC,thereby demonstrating its potential to improve both mechanical and durability properties.展开更多
The selection of appropriate materials for the transportation pipelines is of vital importance to ensure the safety operation in Carbon Capture,Utilisation and Storage(CCUS).To clarify the effects of Cr content in ste...The selection of appropriate materials for the transportation pipelines is of vital importance to ensure the safety operation in Carbon Capture,Utilisation and Storage(CCUS).To clarify the effects of Cr content in steel on the resistance against general and localised corrosion,electrochemistry methods combined with pH measurements and various surface analysis techniques were implemented on X65,1Cr,3Cr and 5Cr steel samples in a CO_(2)-saturated solution at 60°C and pH 6.6 during 192 h of immersion.Additionally,thermodynamic and kinetic analyses of the formation of the corrosion products on carbon steel and low-Cr steels were performed.The results show that the general corrosion resistance increased with rising Cr content without the presence of significant corrosion products formation.However,with the formation and development of the corrosion products,the general corrosion resistance reduced with the increase in Cr content.The formation of the compact crystalline FeCO3 on X65 and 1Cr steel surfaces offered superior general corrosion protection,while cannot provide enough localised corrosion protection.By contrast,the double-structural corrosion product layers on 3Cr and 5Cr steels notably suppressed the localised corrosion,but providing poor protection against general corrosion over long immersion periods.This study reveals the contributions of Cr content on general and localised corrosion resistance at various periods,providing references for material selection and evaluation in CO_(2) environments relevant for CCUS.展开更多
Ni-based catalysts are widely investigated non-noble metal-based systems for CO_(2)methanation.However,their industrial application is still limited due to lower activity at low-temperature and catalyst deactivation.I...Ni-based catalysts are widely investigated non-noble metal-based systems for CO_(2)methanation.However,their industrial application is still limited due to lower activity at low-temperature and catalyst deactivation.Incorporating a second metal such as Ru and Fe is considered as a successful strategy to overcome these challenges through alloy formation or the synergies provided by the interplay of two adjacent metallic sites.Nonetheless,their promotional effect on the CO_(2)methanation mechanism under similar conditions has not been reported yet.In this work,Fe and Ru-promoted Ni/ZrO_(2)catalysts were investigated to evaluate their promotional effect on the mechanism.The Ni/Fe ratio was first optimized and a CO_(2)conversion rate of 37.7 mmolCO_(2)/(molNi+Fes)and 96.3%CH^(4)selectivity was obtained over the Ni_(0.8)Fe_(0.2)/ZrO_(2)catalyst.In comparison with Ni_(0.8)Fe_(0.2)/ZrO_(2),Ni_(0.8)Ru_(0.2)/ZrO_(2)prepared with the same composition showed higher activity and stability in CO_(2)methanation.Characterization results indicate alloys formation and H spillover for Ni_(0.8)Ru_(0.2)/ZrO_(2)to be responsible for promotion.Besides,in situ DRIFTS studies evidenced the occurrence of both CO_(2)dissociative and associative pathways over Ni_(0.8)Ru_(0.2)/ZrO_(2)catalyst,while solely the CO_(2)associative pathway occurred for Ni_(0.8)Fe_(0.2)/ZrO_(2)展开更多
基金the National Natural Science Foundation of China(Grant No.62375032)the Natural Science Foundation of Chongqing(Grant No.CSTB2023TIADKPX0017)+2 种基金the Open Fund of the State Key Laboratory of High Field Laser Physics(Shanghai Institute of Optics and Fine Mechanics)the China Postdoctoral Science Foundation(Grant No.BX20230355)the Department of Education of Guizhou Province(Guizhou Teaching and Technology[2023]015)。
文摘Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion length.However,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical applications.Here,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)reduction.The results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand modulation.Compared with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and CH_(4).The CO and CH_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand modulation.This study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.
基金supported by Hebei Province Higher Education Science and Technology Research Project(No.ZC2024031).
文摘The presence of toxic elements in manganese slag(MSG)poses a threat to the environment due to potential pollution.Utilizing CO_(2) curing on MS offers a promising approach to immobilize toxic substances within this material,thereby mitigating their release into the natural surroundings.This study investigates the impact of CO_(2) cured MS on various rheological parameters,including slump flow,plastic viscosity(η),and yield shear stress(τ).Additionally,it assesses flexural and compressive strengths(f_(t) and f_(cu)),drying shrinkage rates(DSR),durability indicators(chloride ion migration coefficient(CMC),carbonization depth(CD)),and the leaching behavior of heavy metal elements.Microscopic examination via scanning electron microscopy(SEM)is employed to elucidate the underlying mechanisms.The results indicate that CO_(2) curing significantly enhances the slump flow of ultra-high performance concrete(UHPC)by up to 51.2%.Moreover,it reduces UHPC’sηandτby rates ranging from 0%to 52.7%and 0%to 40.2%,respectively.The DSR exhibits a linear increase corresponding to the mass ratio of CO_(2) cured MS.Furthermore,CO_(2) curing enhances both f_(t) and f_(cu) of UHPC by up to 28.7%and 17.6%,respectively.The electrical resistance is also improved,showing an increase of up to 53.7%.The relationship between mechanical strengths and electrical resistance follows a cubic relationship.The CO_(2) cured MS demonstrates a notable decrease in the CMC and CD by rates ranging from 0%to 52.6%and 0%to 26.1%,respectively.The reductions of leached chromium(Cr)and manganese(Mn)are up to 576.3%and 1312.7%,respectively.Overall,CO_(2) curing also enhances the compactness of UHPC,thereby demonstrating its potential to improve both mechanical and durability properties.
基金supported by the National Key R&D Program of China(2021YFB4001601)the Natural Science Foundation of Shandong Province(ZR2021QE036)+3 种基金the Fundamental Research Funds for the Central Universities(22CX06052A)the Postgraduate Innovation Funding Project of China University of Petroleum(East China)(YCX2020070)the Fundamental Research Funds for the Central Universities(20CX02405A)the Development Fund of Shandong Key Laboratory of Oil&Gas Storage and Transportation Safety.
文摘The selection of appropriate materials for the transportation pipelines is of vital importance to ensure the safety operation in Carbon Capture,Utilisation and Storage(CCUS).To clarify the effects of Cr content in steel on the resistance against general and localised corrosion,electrochemistry methods combined with pH measurements and various surface analysis techniques were implemented on X65,1Cr,3Cr and 5Cr steel samples in a CO_(2)-saturated solution at 60°C and pH 6.6 during 192 h of immersion.Additionally,thermodynamic and kinetic analyses of the formation of the corrosion products on carbon steel and low-Cr steels were performed.The results show that the general corrosion resistance increased with rising Cr content without the presence of significant corrosion products formation.However,with the formation and development of the corrosion products,the general corrosion resistance reduced with the increase in Cr content.The formation of the compact crystalline FeCO3 on X65 and 1Cr steel surfaces offered superior general corrosion protection,while cannot provide enough localised corrosion protection.By contrast,the double-structural corrosion product layers on 3Cr and 5Cr steels notably suppressed the localised corrosion,but providing poor protection against general corrosion over long immersion periods.This study reveals the contributions of Cr content on general and localised corrosion resistance at various periods,providing references for material selection and evaluation in CO_(2) environments relevant for CCUS.
基金supported by JARA-Energy(Seed Fund–JARAENERGY MF 005-17 and the joined project“value chains based on CO_(2)”)the Cluster of Excellence Fuel Science Center(EXC 2186,ID:390919832),which is funded by the Excellence Initiative by the German federal and state governments to promote science and research at German universities+1 种基金supported by the National Key Research and Development Program of China(2019YFA0405602)China Scholarship Council(201806420028)。
文摘Ni-based catalysts are widely investigated non-noble metal-based systems for CO_(2)methanation.However,their industrial application is still limited due to lower activity at low-temperature and catalyst deactivation.Incorporating a second metal such as Ru and Fe is considered as a successful strategy to overcome these challenges through alloy formation or the synergies provided by the interplay of two adjacent metallic sites.Nonetheless,their promotional effect on the CO_(2)methanation mechanism under similar conditions has not been reported yet.In this work,Fe and Ru-promoted Ni/ZrO_(2)catalysts were investigated to evaluate their promotional effect on the mechanism.The Ni/Fe ratio was first optimized and a CO_(2)conversion rate of 37.7 mmolCO_(2)/(molNi+Fes)and 96.3%CH^(4)selectivity was obtained over the Ni_(0.8)Fe_(0.2)/ZrO_(2)catalyst.In comparison with Ni_(0.8)Fe_(0.2)/ZrO_(2),Ni_(0.8)Ru_(0.2)/ZrO_(2)prepared with the same composition showed higher activity and stability in CO_(2)methanation.Characterization results indicate alloys formation and H spillover for Ni_(0.8)Ru_(0.2)/ZrO_(2)to be responsible for promotion.Besides,in situ DRIFTS studies evidenced the occurrence of both CO_(2)dissociative and associative pathways over Ni_(0.8)Ru_(0.2)/ZrO_(2)catalyst,while solely the CO_(2)associative pathway occurred for Ni_(0.8)Fe_(0.2)/ZrO_(2)
